具有扩展Hubbard相互作用的铁电钙钛矿氧化物介电性质的第一性原理研究

IF 11.9 1区 材料科学 Q1 CHEMISTRY, PHYSICAL
Min Chul Choi, Wooil Yang, Young-Woo Son, Se Young Park
{"title":"具有扩展Hubbard相互作用的铁电钙钛矿氧化物介电性质的第一性原理研究","authors":"Min Chul Choi, Wooil Yang, Young-Woo Son, Se Young Park","doi":"10.1038/s41524-025-01711-5","DOIUrl":null,"url":null,"abstract":"<p>We investigate the atomic and electronic structures of ferroelectric perovskite oxides, BaTiO<sub>3</sub>, PbTiO<sub>3</sub>, LiNbO<sub>3</sub>, and BiFeO<sub>3</sub> using ab initio extended Hubbard functionals (DFT + <i>U</i> + <i>V</i>), where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli. We compute band structures, ferroelectric distortions, polarization, Born effective charges, and switching barriers, compared with local density approximation, generalized gradient approximation (GGA), meta-GGA, and hybrid (HSE06) functionals. Results from DFT + <i>U</i> + <i>V</i> closely match experimental data, with the inter-site Hubbard terms significantly increasing band gaps, making closer alignment with <i>G</i><i>W</i> results. The crucial role of the inter-site Coulomb interactions, restoring polar distortions suppressed by on-site <i>U</i> is discussed. Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost. This combination of accuracy and efficiency makes DFT + <i>U</i> + <i>V</i> well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.</p>","PeriodicalId":19342,"journal":{"name":"npj Computational Materials","volume":"106 1","pages":""},"PeriodicalIF":11.9000,"publicationDate":"2025-07-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"First principles study of dielectric properties of ferroelectric perovskite oxides with extended Hubbard interactions\",\"authors\":\"Min Chul Choi, Wooil Yang, Young-Woo Son, Se Young Park\",\"doi\":\"10.1038/s41524-025-01711-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>We investigate the atomic and electronic structures of ferroelectric perovskite oxides, BaTiO<sub>3</sub>, PbTiO<sub>3</sub>, LiNbO<sub>3</sub>, and BiFeO<sub>3</sub> using ab initio extended Hubbard functionals (DFT + <i>U</i> + <i>V</i>), where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli. We compute band structures, ferroelectric distortions, polarization, Born effective charges, and switching barriers, compared with local density approximation, generalized gradient approximation (GGA), meta-GGA, and hybrid (HSE06) functionals. Results from DFT + <i>U</i> + <i>V</i> closely match experimental data, with the inter-site Hubbard terms significantly increasing band gaps, making closer alignment with <i>G</i><i>W</i> results. The crucial role of the inter-site Coulomb interactions, restoring polar distortions suppressed by on-site <i>U</i> is discussed. Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost. This combination of accuracy and efficiency makes DFT + <i>U</i> + <i>V</i> well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.</p>\",\"PeriodicalId\":19342,\"journal\":{\"name\":\"npj Computational Materials\",\"volume\":\"106 1\",\"pages\":\"\"},\"PeriodicalIF\":11.9000,\"publicationDate\":\"2025-07-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"npj Computational Materials\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1038/s41524-025-01711-5\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"npj Computational Materials","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1038/s41524-025-01711-5","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

我们使用从头算扩展Hubbard泛函(DFT + U + V)研究了铁电钙钛矿氧化物BaTiO3、PbTiO3、LiNbO3和BiFeO3的原子和电子结构,其中现场和现场间的Hubbard参数是通过Agapito-Curtarolo-Buongiorno Nardelli的伪杂化密度泛函自一致地确定的。我们计算了能带结构、铁电畸变、极化、玻恩有效电荷和开关势垒,并与局部密度近似、广义梯度近似(GGA)、元GGA和混合泛函(HSE06)进行了比较。DFT + U + V的结果与实验数据非常吻合,位点间的Hubbard项显著增加了带隙,与GW的结果更加吻合。讨论了位间库仑相互作用恢复被位间U抑制的极性畸变的关键作用。我们的方法产生了与HSE06相当的精度,计算成本降低了一个数量级以上。这种精度和效率的结合使得DFT + U + V非常适合高通量计算和特性,如铁电异质结构的大块光伏效应和带对准。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

First principles study of dielectric properties of ferroelectric perovskite oxides with extended Hubbard interactions

First principles study of dielectric properties of ferroelectric perovskite oxides with extended Hubbard interactions

We investigate the atomic and electronic structures of ferroelectric perovskite oxides, BaTiO3, PbTiO3, LiNbO3, and BiFeO3 using ab initio extended Hubbard functionals (DFT + U + V), where on-site and inter-site Hubbard parameters are self-consistently determined via a pseudohybrid density functional by Agapito-Curtarolo-Buongiorno Nardelli. We compute band structures, ferroelectric distortions, polarization, Born effective charges, and switching barriers, compared with local density approximation, generalized gradient approximation (GGA), meta-GGA, and hybrid (HSE06) functionals. Results from DFT + U + V closely match experimental data, with the inter-site Hubbard terms significantly increasing band gaps, making closer alignment with GW results. The crucial role of the inter-site Coulomb interactions, restoring polar distortions suppressed by on-site U is discussed. Our approach yields accuracy comparable to HSE06 at over an order-of-magnitude lower computational cost. This combination of accuracy and efficiency makes DFT + U + V well suited for high-throughput calculations and properties such as bulk photovoltaic effect and band alignments of ferroelectric heterostructures.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
npj Computational Materials
npj Computational Materials Mathematics-Modeling and Simulation
CiteScore
15.30
自引率
5.20%
发文量
229
审稿时长
6 weeks
期刊介绍: npj Computational Materials is a high-quality open access journal from Nature Research that publishes research papers applying computational approaches for the design of new materials and enhancing our understanding of existing ones. The journal also welcomes papers on new computational techniques and the refinement of current approaches that support these aims, as well as experimental papers that complement computational findings. Some key features of npj Computational Materials include a 2-year impact factor of 12.241 (2021), article downloads of 1,138,590 (2021), and a fast turnaround time of 11 days from submission to the first editorial decision. The journal is indexed in various databases and services, including Chemical Abstracts Service (ACS), Astrophysics Data System (ADS), Current Contents/Physical, Chemical and Earth Sciences, Journal Citation Reports/Science Edition, SCOPUS, EI Compendex, INSPEC, Google Scholar, SCImago, DOAJ, CNKI, and Science Citation Index Expanded (SCIE), among others.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信